skip to main content
US FlagAn official website of the United States government
dot gov icon
Official websites use .gov
A .gov website belongs to an official government organization in the United States.
https lock icon
Secure .gov websites use HTTPS
A lock ( lock ) or https:// means you've safely connected to the .gov website. Share sensitive information only on official, secure websites.


Title: High-pressure, high-temperature molecular doping of nanodiamond
The development of color centers in diamond as the basis for emerging quantum technologies has been limited by the need for ion implantation to create the appropriate defects. We present a versatile method to dope diamond without ion implantation by synthesis of a doped amorphous carbon precursor and transformation at high temperatures and high pressures. To explore this bottom-up method for color center generation, we rationally create silicon vacancy defects in nanodiamond and investigate them for optical pressure metrology. In addition, we show that this process can generate noble gas defects within diamond from the typically inactive argon pressure medium, which may explain the hysteresis effects observed in other high-pressure experiments and the presence of noble gases in some meteoritic nanodiamonds. Our results illustrate a general method to produce color centers in diamond and may enable the controlled generation of designer defects.  more » « less
Award ID(s):
1719797
PAR ID:
10314904
Author(s) / Creator(s):
; ; ; ; ; ; ;
Date Published:
Journal Name:
Science Advances
Volume:
5
Issue:
5
ISSN:
2375-2548
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
More Like this
  1. Abstract Diamond color centers have been widely studied in the field of quantum optics. The negatively charged silicon vacancy (SiV − ) center exhibits a narrow emission linewidth at the wavelength of 738 nm, a high Debye–Waller factor, and unique spin properties, making it a promising emitter for quantum information technologies, biological imaging, and sensing. In particular, nanodiamond (ND)-based SiV − centers can be heterogeneously integrated with plasmonic and photonic nanostructures and serve as in vivo biomarkers and intracellular thermometers. Out of all methods to produce NDs with SiV − centers, ion implantation offers the unique potential to create controllable numbers of color centers in preselected individual NDs. However, the formation of single color centers in NDs with this technique has not been realized. We report the creation of single SiV − centers featuring stable high-purity single-photon emission through Si implantation into NDs with an average size of ∼20 nm. We observe room temperature emission, with zero-phonon line wavelengths in the range of 730–800 nm and linewidths below 10 nm. Our results offer new opportunities for the controlled production of group-IV diamond color centers with applications in quantum photonics, sensing, and biomedicine. 
    more » « less
  2. Integrating solid-state quantum emitters with photonic circuits is essential for realizing large-scale quantum photonic processors. Negatively charged tin-vacancy (SnV−) centers in diamond have emerged as promising candidates for quantum emitters because of their excellent optical and spin properties, including narrow-linewidth emission and long spin coherence times. SnV− centers need to be incorporated in optical waveguides for efficient onchip routing of the photons they generate. However, such integration has yet to be realized. In this Letter, we demonstrate the coupling of SnV− centers to a nanophotonic waveguide. We realize this device by leveraging our recently developed shallow ion implantation and growth method for the generation of high-quality SnV− centers and the advanced quasi-isotropic diamond fabrication technique. We confirm the compatibility and robustness of these techniques through successful coupling of narrow-linewidth SnV− centers (as narrow as 36 ± 2 MHz) to the diamond waveguide. Furthermore, we investigate the stability of waveguide-coupled SnV− centers under resonant excitation. Our results are an important step toward SnV−-based on-chip spin-photon interfaces, single-photon nonlinearity, and photon-mediated spin interactions. 
    more » « less
  3. Color centers have emerged as a leading qubit candidate for realizing hybrid spin-photon quantum information technology. One major limitation of the platform, however, is that the characteristics of individual color centers are often strain dependent. As an illustrative case, the silicon-vacancy center in diamond typically requires millikelvin temperatures in order to achieve long coherence properties, but strained silicon-vacancy centers have been shown to operate at temperatures beyond 1 K without phonon-mediated decoherence. In this work, we combine high-stress silicon-nitride thin films with diamond nanostructures to reproducibly create statically strained silicon-vacancy color centers (mean ground state splitting of 608 GHz) with strain magnitudes of ∼4×10−4. Based on modeling, this strain should be sufficient to allow for operation of a majority silicon-vacancy centers within the measured sample at elevated temperatures (1.5 K) without any degradation of their spin properties. This method offers a scalable approach to fabricate high-temperature operation quantum memories. Beyond silicon-vacancy centers, this method is sufficiently general that it can be easily extended to other platforms as well. 
    more » « less
  4. Short-pulse ion beams have been developed in recent years and now enable applications in materials science. A tunable flux of selected ions delivered in pulses of a few nanoseconds can affect the balance of defect formation and dynamic annealing in materials. We report results from color center formation in silicon with pulses of 900 keV protons. G-centers in silicon are near-infrared photon emitters with emerging applications as single-photon sources and for spin-photon qubit integration. G-centers consist of a pair of substitutional carbon atoms and one silicon interstitial atom and are often formed by carbon ion implantation and thermal annealing. Here, we report on G-center formation with proton pulses in silicon samples that already contained carbon, without carbon ion implantation or thermal annealing. The number of G-centers formed per proton increased when we increased the pulse intensity from 6.9 × 109 to 7.9 × 1010 protons/cm2/pulse, demonstrating a flux effect on G-center formation efficiency. We observe a G-center ensemble linewidth of 0.1 nm (full width half maximum), narrower than previously reported. Pulsed ion beams can extend the parameter range available for fundamental studies of radiation-induced defects and the formation of color centers for spin-photon qubit applications. 
    more » « less
  5. Abstract The development of high‐quality diamond films is pivotal for driving advances in quantum technology, power electronics, and thermal management. The ion implantation and lift‐off technique has emerged as a crucial method for fabricating diamond films with controlled thickness and scalable production of large‐area diamond wafers. This study advances the understanding of critical interface dynamics during diamond epilayer growth on ion‐implanted commercial diamond substrates. Leveraging high‐resolution cross‐sectional electron microscopy and spectroscopic analyses, the direct transformation of the damaged diamond layer is revealed into a graphitic layer during epilayer overgrowth, eliminating the need for high‐temperature annealing. Raman and photoluminescence spectroscopy mappings along the side section highlight the exceptional quality and purity of the epilayer, showcasing nitrogen‐vacancy center densities comparable to electronic‐grade diamond, making it highly suitable for quantum and electronic applications. Finally, the epilayer detaches efficiently via electrochemical etching, leaving a substrate with low surface roughness that is reusable for multiple growth cycles. These results provide valuable insights into refining the ion implantation and lift‐off process, bridging critical gaps in interface evolution, and establishing a foundation for sustainable, high‐performance diamond films across diverse technological applications. 
    more » « less